| 1. |
- Gamage, Eranga H., et al.
(författare)
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As-Se Pentagonal Linkers to Induce Chirality and Polarity in Mixed-Valent Fe-Se Tetrahedral Chains Resulting in Hidden Magnetic Ordering
- 2022
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Ingår i: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 144:25, s. 11283-11295
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Tidskriftsartikel (refereegranskat)abstract
- A novel mixed-valent hybrid chiral and polar compound, Fe7As3Se12(en)(6)(H2O), has been synthesized by a single-step solvothermal method. The crystal structure consists of 1D [Fe5Se9] chains connected via [As3Se2]-Se pentagonal linkers and charge-balancing interstitial [Fe(en)(3)](2+) complexes (en = ethylenediamine). Neutron powder diffraction verified that interstitial water molecules participate in the crystal packing. Magnetic polarizability of the produced compound was confirmed by X-ray magnetic circular dichroism (XMCD) spectroscopy. X-ray absorption spectroscopy (XAS) and Fe-57 Mossbauer spectroscopy showed the presence of mixed-valent Fe2+/Fe3+ in the Fe-Se chains. Magnetic susceptibility measurements reveal strong antiferromagnetic nearest neighbor interactions within the chains with no apparent magnetic ordering down to 2 K. Hidden short-range magnetic ordering below 70 K was found by Fe-57 Mossbauer spectroscopy, showing that a fraction of the Fe3+/Fe2+ in the chains are magnetically ordered. Nevertheless, complete magnetic ordering is not achieved even at 6 K. Analysis of XAS spectra demonstrates that the fraction of Fe3+ in the chain increases with decreasing temperature. Computational analysis points out several competing ferrimagnetic ordered models within a single chain. This competition, together with variation in the Fe oxidation state and additional weak intrachain interactions, is hypothesized to prevent long-range magnetic ordering.
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| 2. |
- Higley, Daniel J., et al.
(författare)
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Femtosecond X-ray induced changes of the electronic and magnetic response of solids from electron redistribution
- 2019
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Ingår i: Nature Communications. - : Nature Publishing Group. - 2041-1723. ; 10
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Tidskriftsartikel (refereegranskat)abstract
- Resonant X-ray absorption, where an X-ray photon excites a core electron into an unoccupied valence state, is an essential process in many standard X-ray spectroscopies. With increasing X-ray intensity, the X-ray absorption strength is expected to become nonlinear. Here, we report the onset of such a nonlinearity in the resonant X-ray absorption of magnetic Co/Pd multilayers near the Co L-3 edge. The nonlinearity is directly observed through the change of the absorption spectrum, which is modified in less than 40 fs within 2 eV of its threshold. This is interpreted as a redistribution of valence electrons near the Fermi level. For our magnetic sample this also involves mixing of majority and minority spins, due to sample demagnetization. Our findings reveal that nonlinear X-ray responses of materials may already occur at relatively low intensities, where the macroscopic sample is not destroyed, providing insight into ultrafast charge and spin dynamics.
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| 3. |
- Le Guyader, Loïc, et al.
(författare)
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State-resolved ultrafast charge and spin dynamics in [Co/Pd] multilayers
- 2022
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Ingår i: Applied Physics Letters. - : AIP Publishing. - 0003-6951 .- 1077-3118. ; 120:3
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Tidskriftsartikel (refereegranskat)abstract
- We use transient absorption spectroscopy with circularly polarized x rays to detect laser-excited hole states below the Fermi level and compare their dynamics with that of unoccupied states above the Fermi level in ferromagnetic [Co/Pd] multilayers. While below the Fermi level, an instantaneous and significantly stronger demagnetization is observed, above the Fermi level, the demagnetization is delayed by 35 ± 10 fs. This provides a direct visualization of how ultrafast demagnetization proceeds via initial spin-flip scattering of laser-excited holes to the subsequent formation of spin waves.
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| 4. |
- Mandal, Prithwijit, et al.
(författare)
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Orthorhombic distortion drives orbital ordering in the antiferromagnetic 3d1 Mott insulator PrTiO3
- 2023
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Ingår i: Physical Review B. - : American Physical Society (APS). - 2469-9950 .- 2469-9969. ; 108:4
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Tidskriftsartikel (refereegranskat)abstract
- The orbital, which represents the shape of the electron cloud, very often strongly influences the manifestation of various exotic phenomena, e.g., magnetism, metal-insulator transition, colossal magnetoresistance, unconventional superconductivity, etc. in solid-state systems. The observation of the antiferromagnetism in RETiO3 (RE = rare-earth) series has been puzzling since the celebrated Kugel-Khomskii model of spin-orbital superexchange predicts ferromagnetism in an orbitally degenerate d1 system. Further, the existence of the orbitally ordered vs. orbital liquid phase in both antiferromagnetic and paramagnetic phase have been unsettled issues thus far. To address these longstanding questions, we investigate single crystalline film of PrTiO3. Our synchrotron x-ray diffraction measurements confirm the retention of bulklike orthorhombic (D2h) symmetry in the thin film geometry. We observe similar x-ray linear dichroism signal in both paramagnetic and antiferromagnetic phase, which can be accounted by ferro-orbital ordering (FOO). While the presence of D2h crystal field does not guarantee lifting of orbital degeneracy always, we find it to be strong enough in these rare-earth titanates, leading to the FOO state. Thus, our work demonstrates the orthorhombic distortion is the driving force for the orbital ordering of antiferromagnetic RETiO3.
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| 5. |
- Vasiukov, Denis M., et al.
(författare)
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Epitaxial stabilization of thin films of the frustrated Ge-based spinels
- 2021
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Ingår i: Physical Review Materials. - 2475-9953. ; 5:6
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Tidskriftsartikel (refereegranskat)abstract
- Frustrated magnets can host numerous exotic many-body quantum and topological phenomena. GeNi2O4 is a three-dimensional S=1 frustrated magnet with an unusual two-stage transition to the two-dimensional antiferromagnetic ground state, while GeCu2O4 is a high-pressure phase with a strongly tetragonally elongated spinel structure and magnetic lattice formed by S=1/2 CuO2 linear chains with frustrated interchain exchange interactions and exotic magnetic behavior. Here, we report on the thin-film epitaxial stabilization of these two compounds. The developed growth mode, surface morphology, crystal structure, and copper valence state were characterized by in situ reflection high-energy electron diffraction, atomic force microscopy, x-ray reflectivity, x-ray diffraction, x-ray photoelectron spectroscopy, and resonant x-ray absorption spectroscopy. Our results pave an alternative route to the comprehensive investigation of the puzzling magnetic properties of these compounds and the exploration of emergent features driven by strain.
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